Process for the synthesis of izm-2 zeolite in the presence of a template, 1,6-bis(methylpiperidinium)hexane dihydroxide

ABSTRACT

A novel process is described for the preparation of a microporous crystalline solid, known as IZM-2 microporous solid or IZM-2 zeolite. This novel process consists of carrying out the synthesis of IZM-2 zeolite by conversion/transformation of a zeolite with structure type FAU in a fluorinated medium under hydrothermal conditions. In particular, said novel process consists of carrying out the synthesis of an IZM-2 zeolite in a fluorinated medium starting from a zeolite with structure type FAU used as the source of silicon and aluminium and a specific organic molecule or template comprising two quaternary ammonium functions, namely 1,6-bis(methylpiperidinium)hexane dihydroxide.

FIELD OF THE INVENTION

The present invention relates to a novel process for the preparation ofa microporous crystalline solid, termed an IZM-2 microporous solid orIZM-2 zeolite. This novel process consists of carrying out the synthesisof the IZM-2 zeolite by conversion/transformation of a zeolite withstructure type FAU under hydrothermal conditions. In particular, saidnovel process consists of carrying out the synthesis of an IZM-2 zeolitein a fluorinated medium, starting from a zeolite with structure type FAUused as a source of silicon and aluminium and a specific organicmolecule or template comprising two quaternary ammonium functions,namely 1,6-bis(methylpiperidinium)hexane dihydroxide. Said IZM-2microporous solid obtained using the process of the invention isadvantageously of application as a catalyst, adsorbant or separatingagent.

PRIOR ART

Microporous crystalline materials such as zeolites orsilicoaluminophosphates are solids which are widely used in the oilindustry as catalysts, catalyst supports, adsorbants or separationagents. Although many microporous crystalline structures have beendiscovered, the refining and petrochemicals industry is constantlyseeking out novel zeolitic structures which have particular propertiesfor applications such as purification or separation of gases, or theconversion of carbonaceous or other species.

IZM-2 zeolite is a solid with an unknown structure. Model reactions havebeen employed (isomerization and disproportionation of meta-xylenes andisomerization-hydrocracking of n-decane) with the aim of discerning thetopology of the IZM-2 microporous material (Fecant et al. in J. Catal.,20, (2013) 20-29). The results obtained for these reactions indicatethat the structure of the IZM-2 material should be considered to beconstituted by two types of pore sizes (10-MR and 12-MR).

IZM-2 zeolite has been synthesised in its aluminosilicate form (Fecantet al. U.S. Pat. No. 8,361,435 B2) and in its purely silicic form (Li etal. in Microporous Mesoporous Mater., 237 (2017) 222-227), using thequaternary ammonium ion 1,6-bis(methylpiperidinium)hexane as thetemplate, in its hydroxide and bromide form. As far as we are aware, theIZM-2 zeolite was produced using hydroxide anions as the mineralizationagent.

As a general rule, zeolites are prepared by hydrothermal treatment of anaqueous gel containing an amorphous source of silica and aluminium, amineralization agent and a template (Cundy et al. in MicroporousMesoporous Mater., 82 (2005) 1). Recently, a novel operating mode forthe synthesis of zeolite has been described. This means that zeoliticstructures can be produced by hydrothermal synthesis using, as thesource of the reagent, at least one zeolitic structure which will betransformed into another zeolite during the synthesis process. Sano etal. in J. Jpn. Pet. Inst., 56 (2013) 183-197 proposes carrying out thesynthesis of a zeolite with structure type BEA, RUT, CHA, LEV startingfrom a zeolite with structure type FAU using TEAOH (tetraethyl ammoniumhydroxide), TMAOH (tetramethyl ammonium hydroxide), BTMAOH (benzyltrimethyl ammonium hydroxide), Choline (choline hydroxide), respectivelyas the organic molecule; Shi et al. in Microporous Mesoporous Mater.,200 (2014) 269-278 propose carrying out the synthesis of a zeolite withstructure type MWW starting from a zeolite with structure type FAU usingHMI (hexamethyleneimine) as the organic molecule; Goel et al. in Chem.Mater., 27 (2015) 2056-2066 propose carrying out the synthesis of azeolite with structure type MFI starting from a zeolite with structuretype FAU and also a zeolite with structure type BEA using TPABr(tetrapropylammonium bromide) as the organic molecule.

Regarding IZM-2, the only methods known for its preparation consist ofcarrying out a hydrothermal treatment of an aqueous gel containing anamorphous source of silicon and aluminium, an alkaline-earth metal(Na₂O) and a template agent (1,6-bis(methylpiperidinium)hexane).

The present invention concerns a novel process for the preparation of anIZM-2 zeolite by conversion/transformation of a zeolite with structuretype FAU under hydrothermal conditions, in the presence of an organicnitrogen-containing compound or specific template, namely1,6-bis(methylpiperidinium)hexane in its hydroxide form, and for thefirst time in the presence of at least one source of at least onefluoride anion in the synthesis of said zeolite.

In particular, the Applicant has discovered that the nitrogen-containingorganic compound or template 1,6-bis(methylpiperidinium)hexane in itsdihydroxide form, mixed with a zeolite with structure type FAU with amolar ratio SiO_(2 (FAU))/Al₂O_(3 (FAU)) of greater than or equal to 30,used as the source of silicon and of aluminium, in the presence orabsence of a supplemental addition into said mixture of at least onesource of at least one tetravalent element XO₂, and at least one sourceof at least one fluoride anion, leads to the production of a precursorgel for the IZM-2 zeolite with a molar ratio of the total quantity oftetravalent element/Al₂O₃ in the range 10 to 800, the total quantity oftetravalent element representing the sum of the SiO₂ content derivingfrom the FAU zeolite and of the XO₂ content deriving from the additionalsource of an oxide XO₂, in the case in which an addition of at least oneadditional source of an oxide XO₂ is carried out, then to the productionof a high purity IZM-2 zeolite. Any other crystalline or amorphous phaseis generally and highly preferably absent from the crystalline solidconstituting the IZM-2 zeolite obtained from the preparation process.

DESCRIPTION OF THE INVENTION

Thus, the present invention concerns a process for the preparation of anIZM-2 zeolite comprising at least the following steps:

-   -   i) mixing, in an aqueous medium, at least one zeolite with        structure type FAU having a molar ratio        SiO_(2 (FAU))/Al₂O_(3 (FAU)) of greater than or equal to 30, at        least one additional source of an oxide XO₂ in a manner such        that the molar ratio XO₂/SiO_(2 (FAU)) is in the range 0 to 4,        at least one nitrogen-containing organic compound R, R being        1,6-bis(methylpiperidinium)hexane dihydroxide, and at least one        source of at least one fluoride anion, the mixture having the        following molar composition:

(XO₂ + SiO_(2 (FAU)))/ in the range 10 to 800, preferably in the rangeAl₂O_(3 (FAU)) 30 to 600 H₂O/(XO₂ + SiO_(2 (FAU))) in the range 1 to100, preferably in the range 10 to 70, R/(XO₂ + SiO_(2 (FAU))) in therange 0.01 to 0.6, preferably in the range 0.05 to 0.45, BF/(XO₂ +SiO_(2 (FAU))) in the range 0.005 to 0.75, preferably in the range 0.01to 0.65,

-   -   in which X is one or more tetravalent element(s) selected from        the group formed by the following elements: silicon, germanium,        and titanium, preferably silicon, SiO_(2 (FAU)) being the        quantity of SiO₂ supplied by the FAU zeolite, and Al₂O_(3 (FAU))        being the quantity of Al₂O₃ supplied by the FAU zeolite, and in        which BF is selected from fluorine salts in which B is a cation        selected from the cations NH₄ ⁺, Na⁺, K⁺ and Li⁺, and        hydrofluoric acid in aqueous solution,    -   ii) hydrothermal treatment of said mixture obtained from step i)        at a temperature in the range 120° C. to 200° C. for a period in        the range 1 day to 12 days, until said IZM-2 zeolite has been        formed.

Thus, one advantage of the present invention is the provision of a novelpreparation process enabling an IZM-2 zeolite to be formed in afluorinated medium, with high purity starting from a zeolite withstructure type FAU, said process being carried out in the presence of aspecific organic template, namely 1,6-bis(methylpiperidinium)hexanedihydroxide.

Another advantage of the present invention is the provision of a novelprocess for the preparation of a precursor gel of IZM-2 zeolite with aSiO₂/Al₂O₃ molar ratio identical to or superior to the molar ratioSiO_(2 (FAU))/Al₂O_(3 (FAU)) of the starting zeolite with structure typeFAU. The preparation process in accordance with the invention can thusbe used to adjust the SiO₂/Al₂O₃ ratio of the IZM-2 precursor gelobtained as a function of the additional provision or otherwise to thereaction mixture of at least one source of at least one tetravalentelement XO₂.

DETAILED DESCRIPTION OF THE INVENTION

The present invention concerns a process for the preparation of an IZM-2zeolite by the hydrothermal conversion/transformation of a zeolite withstructure type FAU, comprising at least the following steps:

-   -   i) mixing, in an aqueous medium, at least one zeolite with        structure type FAU having a molar ratio        SiO_(2 (FAU))/Al₂O_(3 (FAU)) of greater than or equal to 30, at        least one additional source of an oxide XO₂ in a manner such        that the molar ratio XO₂/SiO_(2 (FAU)) is in the range 0 to 4,        at least one nitrogen-containing organic compound R, R being        1,6-bis(methylpiperidinium)hexane dihydroxide, and at least one        source of at least one fluoride anion, the mixture having the        following molar composition:

(XO₂ + SiO_(2 (FAU)))/ in the range 10 to 800, preferably in the rangeAl₂O_(3 (FAU)) 30 to 600, H₂O/(XO₂ + SiO_(2 (FAU))) in the range 1 to100, preferably in the range 10 to 70, R/(XO₂ + SiO_(2 (FAU))) in therange 0.01 to 0.6, preferably in the range 0.05 to 0.45, BF/(XO₂ +SiO_(2 (FAU))) in the range 0.005 to 0.75, preferably in the range 0.01to 0.65,

-   -   in which X is one or more tetravalent element(s) selected from        the group formed by the following elements: silicon, germanium,        and titanium, preferably silicon, SiO_(2 (FAU)) being the        quantity of SiO₂ supplied by the FAU zeolite, and Al₂O_(3 (FAU))        being the quantity of Al₂O₃ supplied by the FAU zeolite, and in        which BF is selected from fluorine salts in which B is a cation        selected from the cations NH₄ ⁺, Na⁺, K⁺ and Li⁺, and        hydrofluoric acid in aqueous solution,    -   ii) hydrothermal treatment of said mixture obtained from step i)        at a temperature in the range 120° C. to 200° C. for a period in        the range 1 day to 12 days, until said IZM-2 zeolite has been        formed.

In accordance with the invention, a zeolite with structure type FAUhaving a molar ratio SiO_(2 (FAU))/Al₂O_(3 (FAU)) of greater than orequal to 30 preferably in the range 30 and 100 and more preferably inthe range 30 and 80, is incorporated into the mixture as the source ofthe element silicon and aluminium in order to carry out step i).Preferably, said zeolite with structure type FAU is Y zeolite.

In accordance with the invention, the source of the element aluminium issupplied to the mixture for carrying out said step i) of the preparationprocess in accordance with the invention, by the zeolite with structuretype FAU which is used as the source of the element silicon andaluminium.

In accordance with the invention, R is the nitrogen-containing organiccompound R, with R being 1,6-bis(methylpiperidinium)hexane dihydroxide,said compound being incorporated, as the organic template, into themixture in order to carry out step i). The anion associated with thequaternary ammonium cations present in the organic template species forthe synthesis of the solid crystalline IZM-2 in accordance with theinvention is the hydroxide anion.

In accordance with the invention, at least one source of at least onefluoride anion, termed BF, is added to said reaction mixture from stepi), BF being selected from fluorine salts in which B is a cationselected from the cations NH₄ ⁺, Na⁺, K⁺ and Li⁺, and the mixture of atleast two of these salts and hydrofluoric acid in aqueous solution.Preferably, the source of at least one fluoride anion is NH₄F in aqueoussolution.

In accordance with the invention, at least one additional source of anoxide XO₂, X being one or more tetravalent element(s) selected from thegroup formed by the following elements: silicon, germanium, titanium,and preferably silicon, is employed in the mixture of step i) in amanner such that the molar ratio XO₂/SiO_(2 (FAU)) is in the range 0 to4, and preferably in the range 0 and 3, the SiO₂ content in said ratiobeing supplied by the FAU zeolite.

The addition or otherwise of at least one additional source of an oxideXO₂ thus means that the SiO₂/Al₂O₃ ratio of the IZM-2 precursor gelobtained from the mixing step i) can be adjusted in the case in whichX═Si.

The source or sources of said tetravalent element(s) may be any compoundcomprising the element X and which can liberate that element in aqueoussolution in a reactive form. When X is titanium, advantageously Ti(EtO)₄is used as the source of titanium. In the preferred case in which X issilicon, the source of silicon may be any one of said sources routinelyused for the synthesis of zeolites, for example powdered silica, silicicacid, colloidal silica, dissolved silica or tetraethoxysilane (TEOS).Powdered silicas which may be used include precipitated silicas, inparticular those obtained by precipitation from a solution of alkalimetal silicate, fumed silicas, for example “CAB-O-SIL”, and silica gels.It is possible to use colloidal silicas with different particle sizes,for example with a mean equivalent diameter in the range 10 to 15 nm orin the range 40 to 50 nm, such as those marketed under registeredtrademarks such as “LUDOX”. More preferably, the source of silicon isLUDOX HS-40.

In accordance with the invention, the reaction mixture obtained fromstep i) has the following molar composition:

(XO₂ + SiO_(2 (FAU)))/ in the range 10 to 800, preferably in the range30 to Al₂O_(3 (FAU)) 600 and more preferably in the range 80 to 450,H₂O/(XO₂ + in the range 1 to 100, preferably in the range 10 toSiO_(2 (FAU))) 70, and more preferably in the range 15 to 55, R/(XO₂ +in the range 0.01 to 0.6, preferably in the range 0.05 SiO_(2 (FAU))) to0.45, and more preferably in the range 0.085 to 0.4, BF/(XO₂ + in therange 0.005 to 0.75, preferably in the range SiO_(2 (FAU))) 0.01 to0.65, and more preferably in the range 0.02 to 0.55,in which R and BF are as defined above and in which X is one or moretetravalent element(s) selected from the group formed by the followingelements: silicon, germanium, and titanium, preferably silicon, XO₂being the quantity of at least one additional source of an oxide XO₂,SiO_(2 (FAU)) being the quantity of SiO₂ supplied by the FAU zeolite,and Al₂O_(3 (FAU)) being the quantity of Al₂O₃ supplied by the FAUzeolite.

In a preferred embodiment, the mixture of step i) may also contain atleast one source of at least one alkali metal and/or alkaline-earthmetal M with valency n, n being a whole number greater than or equal to1, preferably selected from lithium, potassium, sodium, magnesium andcalcium and a mixture of at least two of these metals. Preferably, thesource of at least one alkali metal and/or alkaline-earth metal issodium hydroxide.

In the preferred embodiment in which the mixture of step i) alsocontains at least the source of at least one alkali metal and/oralkaline-earth metal, the reaction mixture has the following molarcomposition:

(XO₂ + SiO_(2 (FAU)))/Al₂O_(3 (FAU)) in the range 10 to 800, preferablyin the range 80 to 400, H₂O/(XO₂ + SiO_(2 (FAU))) in the range 1 to 100,preferably in the range 10 to 70, R/(XO₂ + SiO_(2 (FAU))) in the range0.01 to 0.6, preferably in the range 0.05 to 0.45, BF/(XO₂ +SiO_(2 (FAU))) in the range 0.005 to 0.75, preferably in the range 0.01to 0.65, M_(2/n)O(XO₂ + SiO_(2 (FAU))) in the range 0.005 to 0.35,preferably in the range 0.01 to 0.3,

-   -   in which X, M, BF, Al₂O_(3 (FAU)), SiO_(2 (FAU)) and XO₂ have        the definitions given above.

Step i) of the process in accordance with the invention consists ofpreparing an aqueous reaction mixture of the IZM-2 zeolite termed aprecursor gel and comprising at least one zeolite with structure typeFAU, optionally a source of an oxide XO₂, at least one organicnitrogen-containing compound R, R being1,6-bis(methylpiperidinium)hexane dihydroxide, in the presence of atleast one source of one or more fluoride salts and/or hydrofluoric acidin aqueous solution. The quantities of said reagents are adjusted in amanner such as to endow this gel with a composition that can allow it tocrystallize into an IZM-2 zeolite.

It may be advantageous to add seeds of IZM-2 zeolite to the reactionmixture during said step i) of the process of the invention in order toreduce the time necessary for the formation of crystals of IZM-2 zeoliteand/or the total crystallization period. Said seeds also promote theformation of said IZM-2 zeolite to the detriment of the impurities. Suchseeds comprise crystalline solids, in particular crystals of IZM-2zeolite. The crystalline seeds are generally added in a proportion inthe range 0.01% to 10% of the mass of the source of at least one oxideof said tetravalent element(s) used in the reaction mixture.

In accordance with step ii) of the process in accordance with theinvention, the gel obtained from step i) undergoes a hydrothermaltreatment, preferably carried out at a temperature in the range 120° C.to 200° C. for a period in the range 1 day to 12 days, until the IZM-2zeolite is formed. The gel is advantageously used under hydrothermalconditions under an autogenous reaction pressure, optionally by adding agas, for example nitrogen, at a temperature which is preferably in therange 120° C. to 195° C., preferably in the range 150° C. to 195° C.,until crystals of IZM-2 zeolite are formed. In accordance with theinvention, the time necessary to obtain crystallization varies between 1day and 12 days, preferably between 2 days and 11 days and morepreferably between 3 days and 10 days. The reaction is generally carriedout with stirring or in the absence of stirring, preferably withstirring.

At the end of the reaction, when said IZM-2 zeolite is formed as aresult of carrying out said step ii) of the preparation process inaccordance with the invention, the solid phase of IZM-2 zeolite which isformed is preferably filtered, washed then dried. Drying is generallycarried out at a temperature in the range 20° C. to 150° C., preferablyin the range 60° C. to 100° C., for a period in the range 5 to 24 hours.The dried zeolite may then advantageously be calcined. The IZM-2zeolite, which has been calcined, is generally analysed by X raydiffraction, this technique also being used to determine the purity ofsaid zeolite obtained by the process of the invention. Highlyadvantageously, the process of the invention results in the formation ofan IZM-2 zeolite, in the absence of any other crystalline or amorphousphases. Said zeolite, after the drying step, is then ready forsubsequent steps such as calcining and ion exchange. For these steps,any of the conventional methods known to the person skilled in the artmay be employed.

The step for calcining the IZM-2 zeolite obtained in accordance with theprocess of the invention is preferably carried out at a temperature inthe range 500° C. to 700° C. for a period in the range 5 to 20 hours.The IZM-2 zeolite obtained from the calcining step is free from anyorganic species, and in particular from the organic template R.

At the end of said calcining step, X ray diffraction can be used toverify that the solid obtained by the process in accordance with theinvention is indeed IZM-2 zeolite. The solid obtained has an X raydiffraction spectrum including at least the peaks recorded in Table 1.

This diffraction spectrum is obtained by radiocrystallographic analysisusing a diffractometer employing the conventional powder technique withthe K_(α1) peak of copper (λ=1.5406 Å). From the position of thediffraction peaks represented by the angle 2θ, the characteristicinterplanar spacings d_(hkl) of the sample are calculated using theBragg relationship. The error in the measurement of d_(hkl), Δ(d_(hkl)),is calculated by the Bragg relationship as a function of the absoluteerror Δ(2θ) in the measurement of 2θ. An absolute error Δ(2θ) of ±0.02°is customarily acceptable. The relative intensity I_(rel) in each valueof d_(hkl) is measured from the height of the corresponding diffractionpeak. The X ray diffraction diagram of the IZM-2 crystalline solid inaccordance with the invention comprises at least the peaks at the valuesof d_(hkl) given in Table 1. In the d_(hkl) column, the mean values ofthe interplanar spacings are shown in Angstroms (Å). Each of thesevalues must be supplemented with an error measurement Δ(d_(hkl)) in therange±0.6 Å to ±0.01 Å.

TABLE 1 Mean values of d_(hkl) and relative intensities measured on an Xray diffraction spectrum of the calcined crystalline solid IZM-2 2 theta(°) d_(hkl) (Å) I_(rel) 7.21 12.25 Mw 7.58 11.66 Mw 8.66 10.21 W 14.696.02 Vw 15.18 5.83 Vw 17.79 4.98 Vw 18.85 4.70 Vw 20.98 4.23 Vs 22.104.02 Mw 22.93 3.88 Mw 23.34 3.81 W 24.24 3.67 Vw 26.24 3.39 Vw 26.543.36 W 27.63 3.23 Vw 29.18 3.06 Vw 32.78 2.73 Vw 36.22 2.48 Vw 38.022.36 Vw 42.63 2.12 Vw 43.57 2.08 W 44.31 2.04 Vwin which: Vs=very strong; S=strong; M=medium; Mw=medium weak; W=weak;Vw=very weak. The relative intensity I_(rel) is given with respect to arelative scale of intensity, in which a value of 100 is attributed tothe most intense peak of the X ray diffraction diagram: Vw<15; 15≤W<30;30≤Mw<50; 50≤M<65; 65≤S<85; Vs≥85.

It is also advantageous to obtain the hydrogen form of the IZM-2 zeoliteobtained by the process in accordance with the invention. Said hydrogenform may be obtained by carrying out an ion exchange with an acid, inparticular a strong mineral acid such as hydrochloric acid, sulphuricacid or nitric acid, or with a compound such as ammonium chloride,sulphate or nitrate. The ion exchange may be carried out by taking upsaid IZM-2 zeolite into suspension in one or more batches with the ionexchange solution. Said zeolite may be calcined before or after the ionexchange, or between two ion exchange steps. Preferably, the zeolite iscalcined before the ion exchange, in order to eliminate any organicsubstance included in the pores of the zeolite, so that ion exchange isfacilitated.

After ion exchange, the IZM-2 zeolite obtained by the process of theinvention may be used as an acidic solid for catalysis in the fields ofrefining and petrochemistry. It may also be used as an adsorbant forcontrolling pollution or as a molecular sieve for separation.

As an example, when it is used as a catalyst, the zeolite prepared inaccordance with the process of the invention is calcined, exchanged andis preferably in the hydrogen form, and may be associated with aninorganic matrix which may be inert or catalytically active, and with ametallic phase. The inorganic matrix may be present simply as a binderin order to keep the small particles of the zeolite together in thevarious known forms for catalysts (extrudates, pellets, beads, powders),or in fact it may be added as a diluent in order to impose the degree ofconversion in a process which would otherwise occur at too fast a rate,leading to clogging of the catalyst as a result of too much cokeformation. Typical inorganic matrices are in particular supportmaterials for the catalysts, such as silica, the various forms ofalumina, magnesia, zirconia, oxides of titanium, boron, titanium,zirconium, aluminium phosphates, kaolinic clays, bentonites,montmorillonites, sepiolite, attapulgite, Fuller's earth, syntheticporous materials such as SiO₂—Al₂O₃, SiO₂—ZrO₂, SiO₂—ThO₂, SiO₂—BeO,SiO₂—TiO₂, or any combination of these compounds. The inorganic matrixmay be a mixture of different compounds, in particular of an inert phaseand an active phase.

The zeolite prepared in accordance with the process of the invention mayalso be associated with at least one other zeolite and act as theprincipal active phase or the additive.

The metallic phase is introduced onto the zeolite alone, the inorganicmatrix alone or the inorganic matrix-zeolite assembly by ion exchange orimpregnation with cations or oxides selected from the followingelements: Cu, Ag, Ga, Mg, Ca, Sr, Zn, Cd, B, Al, Sn, Pb, V, P, Sb, Cr,Mo, W, Mn, Re, Fe, Co, Ni, Pt, Pd, Ru, Rh, Os, Ir and any other elementfrom the periodic classification of the elements. The metals may beintroduced either all in the same manner, or using different techniques,at any point of the preparation, before or after shaping and in anyorder. In addition, intermediate treatments such as, for example,calcining and/or reduction, may be applied between deposits of thevarious metals.

The catalytic compositions comprising the IZM-2 zeolite prepared inaccordance with the process of the invention are in general suitable forcarrying out the principal processes for the transformation ofhydrocarbons and reactions for the synthesis of organic compounds suchas ethers.

Any method for shaping which is known to the person skilled in the artis suitable for the catalyst comprising the IZM-2 zeolite. As anexample, it may be possible to use pelletization or extrusion, orshaping into beads. The shaping of the catalyst containing the zeoliteprepared in accordance with the process of the invention and being atleast in part in the acidic form is generally such that the catalyst ispreferably in the form of extrudates or beads with a view to their use.

Without further elaboration, it is believed that one skilled in the artcan, using the preceding description, utilize the present invention toits fullest extent. The preceding preferred specific embodiments are,therefore, to be construed as merely illustrative, and not limitative ofthe remainder of the disclosure in any way whatsoever.

In the foregoing and in the examples, all temperatures are set forthuncorrected in degrees Celsius and, all parts and percentages are byweight, unless otherwise indicated.

The entire disclosures of all applications, patents and publications,cited herein and of corresponding application No. FR 1752472, filed Mar.24, 2017 are incorporated by reference herein.

The invention will now be illustrated in the following examples, whichare not in any case limiting in nature.

Example 1: Preparation of 1,6-Bis(Methylpiperidinium) Hexane Dihydroxide(R(OH)2 Template) Starting from 1,6-Bis(Methylpiperidinium) HexaneDibromide

50 g of 1,6-dibromohexane (0.20 mole, 99%, Alfa Aesar) was added to a 1L flask containing 50 g of N-methylpiperidine (0.51 mole, 99%, AlfaAesar) and 200 mL of ethanol. The reaction medium was stirred and heatedunder reflux for 5 h. The mixture was then cooled to ambient temperatureand filtered. The mixture was poured into 300 mL of cold diethylether,then the precipitate formed was filtered and washed with 100 mL ofdiethylether. The solid obtained was recrystallized from anethanol/ether mixture. The solid obtained was dried under vacuum for 12h. 71 g of a white solid was obtained (i.e. a yield of 80%).

The product had the expected ¹H NMR spectrum. ¹H NMR (D₂O, ppm/TMS):1.27 (4H, m); 1.48 (4H, m); 1.61 (4H, m); 1.70 (8H, m); 2.85 (6H, s);3.16 (12H, m).

18.9 g of Ag₂O (0.08 mole, 99%, Aldrich) was added to a 250 mL Teflonbeaker containing 30 g of the 1,6-bis(methylpiperidinium) dibromidetemplate (0.07 mole) prepared in accordance with Example 1 and 100 mL ofdeionized water. The reaction medium was stirred in the absence of lightfor 12 h. The mixture was then filtered. The filtrate obtained wascomposed of an aqueous solution of 1,6-bis(methylpiperidinium)hexanedihydroxide. This species was assayed by proton NMR using formic acidfor calibration.

Example 2: Preparation of an IZM-2 Solid in Accordance with theInvention

51 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 1621.3 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2, and stirring of the mixture wasmaintained for 10 minutes. In order to promote the formation of thecrystalline solid IZM-2, 5 mg of IZM-2 zeolite seeds was added to thesynthesised mixture and stirring was maintained for 5 minutes. 342.6 mgof colloidal silica (Ludox HS40, 40% by weight, Aldrich) wasincorporated into the synthesised mixture and stirring was maintainedfor 15 minutes. 575 mg of an aqueous solution containing 10% by weightof ammonium fluoride (≥99.9% by weight, Aldrich) was incorporated intothe synthesised mixture, and stirring was maintained for the timenecessary to evaporate the solvent until the desired concentration forthe gel was obtained, i.e. the molar composition of the mixture was asfollows: 1 SiO₂: 0.0033 Al₂O₃: 0.33 R(OH)₂: 0.5 NH₄F: 33.33 H₂O, i.e. aSiO₂/Al₂O₃ ratio of 300. The mixture was then transferred into anautoclave following homogenization. The autoclave was closed then heatedfor 8 days at 170° C., with stirring. The crystalline product obtainedwas filtered, washed with deionized water then dried overnight at 100°C. The solid was then introduced into a muffle furnace in which acalcining step was carried out: the calcining cycle comprised a rise intemperature to 200° C., a constant temperature stage at 200° C.maintained for 2 hours, a rise in temperature to 550° C. followed by aconstant temperature stage at 550° C. maintained for 8 hours, followedby a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 3: Preparation of an IZM-2 Solid in Accordance with theInvention

51 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 1228.2 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 630 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.In order to promote the formation of the crystalline solid IZM-2, 5 mgof IZM-2 zeolite seeds was added to the synthesised mixture and stirringwas maintained for 5 minutes. 342.6 mg of colloidal silica (Ludox HS40,40% by weight, Aldrich) was incorporated into the synthesised mixtureand stirring was maintained for 15 minutes. 58 mg of an aqueous solutioncontaining 10% by weight of ammonium fluoride (≥99.9% by weight,Aldrich) was incorporated into the synthesised mixture, and stirring wasmaintained for the time necessary to evaporate the solvent until thedesired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.0033 Al₂O₃: 0.25R(OH)₂: 0.05 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 300. Themixture was then transferred into an autoclave following homogenization.The autoclave was closed then heated for 8 days at 170° C., withstirring. The crystalline product obtained was filtered, washed withdeionized water then dried overnight at 100° C. The solid was thenintroduced into a muffle furnace in which a calcining step was carriedout: the calcining cycle comprised a rise in temperature to 200° C., aconstant temperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 4: Preparation of an IZM-2 Solid in Accordance with theInvention

51 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 412 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 513 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.In order to promote the formation of the crystalline solid IZM-2, 5 mgof IZM-2 zeolite seeds was added to the synthesised mixture and stirringwas maintained for 5 minutes. 109 mg of colloidal silica (Ludox HS40,40% by weight, Aldrich) was incorporated into the synthesised mixtureand stirring was maintained for 15 minutes. 29 mg of an aqueous solutioncontaining 10% by weight of ammonium fluoride (≥99.9% by weight,Aldrich) was incorporated into the synthesised mixture and stirring wasmaintained for the time necessary to evaporate the solvent until thedesired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.0066 Al₂O₃: 0.17R(OH)₂: 0.05 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 150. Themixture was then transferred into an autoclave following homogenization.The autoclave was closed then heated for 8 days at 170° C., withstirring. The crystalline product obtained was filtered, washed withdeionized water then dried overnight at 100° C. The solid was thenintroduced into a muffle furnace in which a calcining step was carriedout: the calcining cycle comprised a rise in temperature to 200° C., aconstant temperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2. The diffraction spectrumfor the calcined solid IZM-2 is given in FIG. 1.

Example 5: Preparation of an IZM-2 Solid in Accordance with theInvention

51 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 412 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 453 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.In order to promote the formation of the crystalline solid IZM-2, 5 mgof seeds of the IZM-2 zeolite was added to the synthesised mixture andstirring was maintained for 5 minutes. 109 mg of colloidal silica (LudoxHS40, 40% by weight, Aldrich) was incorporated into the synthesisedmixture and stirring was maintained for 15 minutes. 96 mg of an aqueoussolution containing 10% by weight of ammonium fluoride (≥99.9% byweight. Aldrich) was incorporated into the synthesised mixture andstirring was maintained for the time necessary to evaporate the solventuntil the desired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.0066 Al₂O₃: 0.17R(OH)₂: 0.17 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 150. Themixture was then transferred into an autoclave following homogenization.The autoclave was closed then heated for 8 days at 170° C., withstirring. The crystalline product obtained was filtered, washed withdeionized water then dried overnight at 100° C. The solid was thenintroduced into a muffle furnace in which a calcining step was carriedout: the calcining cycle comprised a rise in temperature to 200° C., aconstant temperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 6: Preparation of an IZM-2 Solid in Accordance with theInvention

90 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 485.1 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 649 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.In order to promote the formation of the crystalline solid IZM-2, 9 mgof IZM-2 zeolite seeds was added to the synthesised mixture and stirringwas maintained for 5 minutes. 55 mg of colloidal silica (Ludox HS40, 40%by weight, Aldrich) was incorporated into the synthesised mixture andstirring was maintained for 15 minutes. 34 mg of an aqueous solutioncontaining 10% by weight of ammonium fluoride (≥99.9% by weight Aldrich)was incorporated into the synthesised mixture, and stirring wasmaintained for the time necessary to evaporate the solvent until thedesired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.01 Al₂O₃: 0.17R(OH)₂: 0.05 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 100. Themixture was then transferred into an autoclave following homogenization.The autoclave was closed then heated for 8 days at 170° C., withstirring. The crystalline product obtained was filtered, washed withdeionized water then dried overnight at 100° C. The solid was thenintroduced into a muffle furnace in which a calcining step was carriedout: the calcining cycle comprised a rise in temperature to 200° C., aconstant temperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 7: Preparation of an IZM-2 Solid in Accordance with theInvention

90 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 954.6 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 1 mg of deionized water.Stirring of the mixture obtained was maintained for 10 minutes. In orderto promote the formation of the crystalline solid IZM-2, 9 mg of IZM-2zeolite seeds was added to the synthesised mixture and stirring wasmaintained for 5 minutes. 55 mg of colloidal silica (Ludox HS40, 40% byweight, Aldrich) was incorporated into the synthesised mixture andstirring was maintained for 15 minutes. 339 mg of an aqueous solutioncontaining 10% by weight of ammonium fluoride (≥99.9% by weight,Aldrich) was incorporated into the synthesised mixture, and stirring wasmaintained for the time necessary to evaporate the solvent until thedesired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.01 Al₂O₃: 0.33R(OH)₂: 0.5 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 100. The mixturewas then transferred into an autoclave following homogenization. Theautoclave was closed then heated for 8 days at 170° C., with stirring.The crystalline product obtained was filtered, washed with deionizedwater then dried overnight at 100° C. The solid was then introduced intoa muffle furnace in which a calcining step was carried out: thecalcining cycle comprised a rise in temperature to 200° C., a constanttemperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 8: Preparation of an IZM-2 Solid in Accordance with theInvention

90 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 723.2 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 388 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.In order to promote the formation of the crystalline solid IZM-2, 9 mgof IZM-2 zeolite seeds was added to the synthesised mixture and stirringwas maintained for 5 minutes. 55 mg of colloidal silica (Ludox HS40, 40%by weight, Aldrich) was incorporated into the synthesised mixture andstirring was maintained for 15 minutes. 113 mg of an aqueous solutioncontaining 10% by weight of ammonium fluoride (≥99.9% by weight,Aldrich) was incorporated into the synthesised mixture, and stirring wasmaintained for the time necessary to evaporate the solvent until thedesired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.01 Al₂O₃: 0.25R(OH)₂: 0.17 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 100. Themixture was then transferred into an autoclave following homogenization.The autoclave was closed then heated for 8 days at 170° C., withstirring. The crystalline product obtained was filtered, washed withdeionized water then dried overnight at 100° C. The solid was thenintroduced into a muffle furnace in which a calcining step was carriedout: the calcining cycle comprised a rise in temperature to 200° C., aconstant temperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 9: Preparation of an IZM-2 Solid in Accordance with theInvention

90 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 436.7 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 597 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.In order to promote the formation of the crystalline solid IZM-2, 9 mgof IZM-2 zeolite seeds was added to the synthesised mixture and stirringwas maintained for 5 minutes. 27.5 mg of colloidal silica (Ludox HS40,40% by weight, Aldrich) was incorporated into the synthesised mixtureand stirring was maintained for 15 minutes. 30 mg of an aqueous solutioncontaining 10% by weight of ammonium fluoride (≥99.9% by weight,Aldrich) was incorporated into the synthesised mixture, and stirring wasmaintained for the time necessary to evaporate the solvent until thedesired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.011 Al₂O₃: 0.17R(OH)₂: 0.05 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 90. The mixturewas then transferred into an autoclave following homogenization. Theautoclave was closed then heated for 8 days at 170° C., with stirring.The crystalline product obtained was filtered, washed with deionizedwater then dried overnight at 100° C. The solid was then introduced intoa muffle furnace in which a calcining step was carried out: thecalcining cycle comprised a rise in temperature to 200° C., a constanttemperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 10: Preparation of an IZM-2 Solid in Accordance with theInvention

90 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 436.7 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 533 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.In order to promote the formation of the crystalline solid IZM-2, 9 mgof IZM-2 zeolite seeds was added to the synthesised mixture and stirringwas maintained for 5 minutes. 27.5 mg of colloidal silica (Ludox HS40,40% by weight, Aldrich) was incorporated into the synthesised mixtureand stirring was maintained for 15 minutes. 102 mg of an aqueoussolution containing 10% by weight of ammonium fluoride (≥99.9% byweight, Aldrich) was incorporated into the synthesised mixture, andstirring was maintained for the time necessary to evaporate the solventuntil the desired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.011 Al₂O₃: 0.17R(OH)₂: 0.17 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 90. The mixturewas then transferred into an autoclave following homogenization. Theautoclave was closed then heated for 8 days at 170° C., with stirring.The crystalline product obtained was filtered, washed with deionizedwater then dried overnight at 100° C. The solid was then introduced intoa muffle furnace in which a calcining step was carried out: thecalcining cycle comprised a rise in temperature to 200° C., a constanttemperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 11: Preparation of an IZM-2 Solid in Accordance with theInvention

90 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 859.3 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 14 mg of deionized water.Stirring of the mixture obtained was maintained for 10 minutes. In orderto promote the formation of the crystalline solid IZM-2, 9 mg of IZM-2zeolite seeds was added to the synthesised mixture and stirring wasmaintained for 5 minutes. 27.5 mg of colloidal silica (Ludox HS40, 40%by weight, Aldrich) was incorporated into the synthesised mixture andstirring was maintained for 15 minutes. 305 mg of an aqueous solutioncontaining 10% by weight of ammonium fluoride (≥99.9% by weight,Aldrich) was incorporated into the synthesised mixture, and stirring wasmaintained for the time necessary to evaporate the solvent until thedesired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.011 Al₂O₃: 0.33R(OH)₂: 0.5 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 90. The mixturewas then transferred into an autoclave following homogenization. Theautoclave was closed then heated for 8 days at 170° C., with stirring.The crystalline product obtained was filtered, washed with deionizedwater then dried overnight at 100° C. The solid was then introduced intoa muffle furnace in which a calcining step was carried out: thecalcining cycle comprised a rise in temperature to 200° C., a constanttemperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 12: Preparation of an IZM-2 Solid in Accordance with theInvention

90 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 388.2 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 488 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.In order to promote the formation of the crystalline solid IZM-2, 9 mgof IZM-2 zeolite seeds was added to the synthesised mixture and stirringwas maintained for 5 minutes. 90 mg of an aqueous solution containing10% by weight of ammonium fluoride (≥99.9% by weight, Aldrich) wasincorporated into the synthesised mixture, and stirring was maintainedfor the time necessary to evaporate the solvent until the desiredconcentration for the gel was obtained, i.e. the molar composition ofthe mixture was as follows: 1 SiO₂: 0.013 Al₂O₃: 0.17 R(OH)₂: 0.17 NH₄F:33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 80. The mixture was thentransferred into an autoclave following homogenization. The autoclavewas closed then heated for 8 days at 170° C., with stirring. Thecrystalline product obtained was filtered, washed with deionized waterthen dried overnight at 100° C. The solid was then introduced into amuffle furnace in which a calcining step was carried out: the calciningcycle comprised a rise in temperature to 200° C., a constant temperaturestage at 200° C. maintained for 2 hours, a rise in temperature to 550°C. followed by a constant temperature stage at 550° C. maintained for 8hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 13: Preparation of an IZM-2 Solid in Accordance with theInvention

90 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 763.9 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 27 mg of deionized water.Stirring of the mixture obtained was maintained for 10 minutes. In orderto promote the formation of the crystalline solid IZM-2, 9 mg of IZM-2zeolite seeds was added to the synthesised mixture and stirring wasmaintained for 5 minutes. 271 mg of an aqueous solution containing 10%by weight of ammonium fluoride (≥99.9% by weight, Aldrich) wasincorporated into the synthesised mixture, and stirring was maintainedfor the time necessary to evaporate the solvent until the desiredconcentration for the gel was obtained, i.e. the molar composition ofthe mixture was as follows: 1 SiO₂: 0.013 Al₂O₃: 0.33 R(OH)₂: 0.5 NH₄F:33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of 80. The mixture was thentransferred into an autoclave following homogenization. The autoclavewas closed then heated for 8 days at 170° C., with stirring. Thecrystalline product obtained was filtered, washed with deionized waterthen dried overnight at 100° C. The solid was then introduced into amuffle furnace in which a calcining step was carried out: the calciningcycle comprised a rise in temperature to 200° C., a constant temperaturestage at 200° C. maintained for 2 hours, a rise in temperature to 550°C. followed by a constant temperature stage at 550° C. maintained for 8hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

Example 14: Preparation of an IZM-2 Solid in Accordance with theInvention

54 mg of a zeolite with structure type FAU (CBV780, SiO₂/Al₂O₃=80,Zeolyst) was mixed with 650.3 mg of an aqueous solution of1,6-bis(methylpiperidinium)hexane dihydroxide (20.04% by weight)prepared in accordance with Example 2 and with 896 mg of deionizedwater. Stirring of the mixture obtained was maintained for 10 minutes.82 mg of an aqueous solution containing 20% by weight of sodiumhydroxide (98% by weight, Aldrich) was added. In order to promote theformation of the crystalline solid IZM-2, 5 mg of IZM-2 zeolite seedswas added to the synthesised mixture and stirring was maintained for 15minutes. 362.7 mg of colloidal silica (Ludox HS40, 40% by weight,Aldrich) was incorporated into the synthesised mixture. Finally, 305 mgof an aqueous solution containing 10% by weight of ammonium fluoride(≥99.9% by weight Aldrich) was added and stirring of the mixture wasmaintained for the time necessary to evaporate the solvent until thedesired concentration for the gel was obtained, i.e. the molarcomposition of the mixture was as follows: 1 SiO₂: 0.0033 Al₂O₃: 0.125R(OH)₂: 0.0625 Na₂O: 0.25 NH₄F: 33.33 H₂O, i.e. a SiO₂/Al₂O₃ ratio of300. The mixture was then transferred into an autoclave followinghomogenization. The autoclave was closed then heated for 6 days at 170°C., with stirring. The crystalline product obtained was filtered, washedwith water then dried overnight at 100° C. The solid was then introducedinto a muffle furnace in which a calcining step was carried out: thecalcining cycle comprised a rise in temperature to 200° C., a constanttemperature stage at 200° C. maintained for 2 hours, a rise intemperature to 550° C. followed by a constant temperature stage at 550°C. maintained for 8 hours, followed by a return to ambient temperature.

The calcined solid product was analysed by X ray diffraction andidentified as being constituted by solid IZM-2.

The preceding examples can be repeated with similar success bysubstituting the generically or specifically described reactants and/oroperating conditions of this invention for those used in the precedingexamples.

From the foregoing description, one skilled in the art can easilyascertain the essential characteristics of this invention and, withoutdeparting from the spirit and scope thereof, can make various changesand modifications of the invention to adapt it to various usages andconditions.

1. Process for the preparation of an IZM-2 zeolite, comprising at leastthe following steps: i) mixing, in an aqueous medium, at least onezeolite with structure type FAU having a molar ratioSiO_(2 (FAU))/Al₂O_(3 (FAU)) of greater than or equal to 30, at leastone additional source of an oxide XO₂ in a manner such that the molarratio XO₂/SiO_(2 (FAU)) is in the range 0 to 4, at least onenitrogen-containing organic compound R, R being1,6-bis(methylpiperidinium)hexane dihydroxide, and at least one sourceof at least one fluoride anion, the mixture having the following molarcomposition: (XO₂ + SiO_(2 (FAU)))/Al₂O_(3 (FAU)) in the range 30 to600, H₂O/(XO₂ + SiO_(2 (FAU))) in the range 1 to 100, R/(XO₂ +SiO_(2 (FAU))) in the range 0.01 to 0.6, BF/(XO₂ + SiO_(2 (FAU))) in therange 0.005 to 0.75,

in which X is one or more tetravalent element(s) selected from the groupformed by the following elements: silicon, germanium, and titanium,preferably silicon, SiO_(2 (FAU)) being the quantity of SiO₂ supplied bythe FAU zeolite, and Al₂O_(3 (FAU)) being the quantity of Al₂O₃ suppliedby the FAU zeolite, and in which BF is selected from fluorine salts inwhich B is a cation selected from the cations NH₄ ⁺, Na⁺, K⁺ and Li⁺,and hydrofluoric acid in aqueous solution, ii) hydrothermal treatment ofsaid mixture obtained from step i) at a temperature in the range 120° C.to 200° C. for a period in the range 1 day to 10 days, until said IZM-2zeolite has been formed.
 2. The process as claimed in claim 1, in whichsaid zeolite with structure type FAU is Y zeolite.
 3. The process asclaimed in claim 1, in which the source BF of at least one anion is NH₄Fin aqueous solution.
 4. The process as claimed in claim 1, in which X issilicon.
 5. The process as claimed in claim 1, in which the additionalsource of an oxide XO₂ is added in the mixing step i) in a manner suchthat the molar ratio XO₂/SiO_(2 (FAU)) is in the range 0 to
 3. 6. Theprocess as claimed in claim 1, in which the reaction mixture obtained instep i) has the following molar composition: (XO₂ +SiO_(2 (FAU)))/Al₂O_(3 (FAU)) in the range 30 to 600, H₂O/(XO₂ +SiO_(2 (FAU))) in the range 10 to 70, R/(XO₂ + SiO_(2 (FAU))) in therange 0.05 to 0.45, BF/(XO₂ + SiO_(2 (FAU))) in the range 0.01 to 0.65.


7. The process as claimed in claim 6, in which the reaction mixtureobtained in step i) has the following molar composition: (XO₂ +SiO_(2 (FAU)))/Al₂O_(3 (FAU)) in the range 80 to 450, H₂O/(XO₂ +SiO_(2 (FAU))) in the range 15 to 55 R/(XO₂ + SiO_(2 (FAU))) in therange 0.085 to 0.4 BF/(XO₂ + SiO_(2 (FAU))) in the range 0.02 to 0.55.


8. The process as claimed in claim 1, in which the mixture of step i)also contains at least one source of at least one alkali metal and/oralkaline-earth metal M with valency n, n being a whole number greaterthan or equal to 1, selected from lithium, potassium, sodium, magnesiumand calcium and a mixture of at least two of these metals.
 9. Theprocess as claimed in claim 1, in which the hydrothermal treatment ofstep ii) is carried out at a temperature in the range 120° C. to 195° C.10. The process as claimed in claim 1, in which the hydrothermaltreatment of step ii) is carried out for a period in the range 2 days to11 days.